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1.
Individual aerosol particles collected in the Negev desert in Israel during a summer and winter campaign in 1996–1997 were analysed by scanning electron microscopy with energy-dispersive X-ray analysis. Hierarchical cluster analysis was performed to interpret the data on the basis of particle diameter and composition. Eleven particle classes (groups) provided clues on sources and/or particle formation. The summer samples were enriched in sulphates and mineral dusts; the winter samples contained more sea salts, aged sea salts, and industrial particles. The fine size fraction below 1 m diameter was enriched in secondary particles and showed evidence of atmospheric processing. The secondary sulphate particles were mainly attributed to long-range transport. A regional conversion from calcite to calcium sulphate occurred during summer. Industrial particles originating from local pollution appeared during winter.  相似文献   

2.
A method for determining the distribution of supermicrometer nitrate between size-segregated sea-salt and soil derived particles is presented. The analysis is based on field data from six measurements at a coastal site in southern Finland, and on a theoretical treatment taking into account the transfer of gaseous species onto particle surfaces and their subsequent reaction. Significant amounts of nitrate were found in both the particle types, with the fraction of nitrate associated with soil particles varying from 20–50% in the 1–2 m size to near 90% in particles larger than 10 m. Overall, the nitrate accumulation followed closely the relative abundances of these two particle types. Two overlapping modes in supermicron nitrate mass size distributions could be identified. The lower mode, associated with sea-salt, was located between the surface-area and volume distribution of sodium peaking at about 2–3 m of EAD. The upper mode peaked at 3–5 m and followed more closely the surface-area distribution of calcium in all samples. At our site, the accumulation of nitrate into both particle types was shown to be limited by an effective surface reaction rate rather than by gas-phase diffusion. This rate was estimated to be considerably larger for sea-salt particles. Strong evidence in support of the saturation of nitrate in sea-salt particles were obtained.  相似文献   

3.
Fourteen samples of fresh falling snow were collected at Antarctic coastal base Dumont d'Urville in 1984. The samples have been analysed for major ions (including MSA) by ion chromatography and acid titration. The results are relevant to the chemical composition of background precipitation in polar marine conditions. The seasalt aerosol contribution is dominant. All samples are found to be acidic in the range 3–16 eq/l. The calculated non-seasalt sulfate (nssSO4 2-) concentration is significantly negative for 3 of the 14 samples. NssSO4 2- is found to be relatively high in summer and fall. MSA also exhibits the same pattern probably linked to local marine biogenic activity and/or atmospheric photochemical processes. The MSA to nssSO4 2- ratio is in good agreement with values reported for coastal Antarctic ice cores and subantarctic acrosol. The background mean value for nitrate concentration is 1.1 eq/l but two very strong spikes (up to 16 eq/l) are observed. The first seems to be linked with long range transport of continental air masses while the second (in winter) is clearly due to a sudden input of nitric acid, possibly from the stratosphere.This paper represents a preliminary approach to a larger air and snow monitoring to be developped at this site.  相似文献   

4.
Thermal and optical techniques were used at Barrow, Alaska during AGASP II (3/20/86–4/7/86) to measure in-situ variability of major aerosol components present in Arctic Haze. The experiment provided continuous data on the concentration, size distribution and relative proportions of sulfate species and refractory aerosol for particle diameters of 0.15 to 5 m. Filter samples were also taken for determination of aerosol optical absorption due to soot (EC-elemental carbon). Although pronounced haze events were absence during this period the haze aerosol present varied in concentration between 2 and 6 g/m3 but showed little change in relative constituents. Apart from local influences, the optical data indicated a persistent fine-mode sulfate aerosol with a NH4 +/SO4 – molar ratio of about 0.4 and a refractory component of somewhat less than 10% by mass. A preliminary comparison of soot estimates determined from the light absorption data with the size distributions of refractory aerosol observed independently by the optical particle counter showed good agreement during the sample period. In the absence of local pollution, values of single scatter albedo derived from light scattering and light absorption showed similar variation about the average value of 0.86 found by us during flights north of Barrow three years earlier during AGASP I.  相似文献   

5.
Systematic year-round observations of submicron aerosols were carried out at Syowa Station (69°00'S, 39°35'E) in 1978. On the basis of the results of these observations, it is concluded that two types of aerosols originating from different sources are present in the Antarctic croposphere. With the intrusion of maritime air, mostly in the polar night months, sea salt particles and ammonium sulfate particles contained originally in the clean maritime air are dominant. The size distribution of such aerosols is monomodal, having a single mode at around 0.03 m in radii. On the other hand, in the sunlit months, sulfuric acid droplets are predominant and the size distribution is bimodal, having an additional mode at around 0.005 m in radii. Those sulfuric acid particles seem to be formed photochemically within a specific layer in the mid to lower troposphere over Antarctica. Most Antarctic submicron particles are of tropospheric origin, not of stratospheric nor anthropogenic origin.  相似文献   

6.
Levels of formate and acetate in dew were measured at Dayalbagh, India, usingsurrogate surfaces. The dew formed per night ranged between 0.06 lm–2 and 1.38 l m–2, with an average of 0.59l m–2. pH ranged between 6.7 and 7.4. Mean concentrations offormate and acetate in dew were 10.2 ± 10.2 eql–1 and 7.5 ± 4.5 eq l–1,respectively. The correlation coefficient between the two ions was 0.80 (p =0.001), which suggested that concentrations of these species in dew are linkedtogether. They have either common or different sources with fairly constantstrengths or products of same reaction. Good correlation of formate andacetate with Ca (r = 0.82 and r = 0.70, respectively) and Mg (r = 0.74 and r= 0.71, respectively) suggested that these ions may be associated with Ca andMg after the neutralization process. Deposition rates for formate and acetatein dew per night were 10.2 ± 7.22 mol m–2 pernight and 4.6 ± 2.2 mol m–2 per night,respectively. The theoretical Henry's law constant (K* H)and the field-observed Henry's law coefficient (K* H) ascalculated from concurrent measurements of gas phase and dew for both acidsshowed large discrepancies of three orders of magnitude.  相似文献   

7.
Cascade impactor samples were collected over the Alaskan Arctic during the first three research flights of AGASP-II. These samples were analyzed using analytical electron microscopy to determine the morphology, mineralogy and elemental composition of individual particles. For analytical considerations, a typical impactor sample was run for approximately 20 min, thus giving excellent time resolution of discrete events.Samples collected during flights 201 and 202 consisted of stratospheric aerosol and lower-altitude haze samples. Stratospheric samples were characterized by moderate loadings of H2SO4 droplets with relatively few particles of other types. Samples collected in tropospheric haze layers generally exhibited light-to-moderate particle loadings. H2SO4 was again the most prevalent species, with crustal and anthropogenic particles also observed. One sample taken over south-central Alaska near the end of flight 203 showed high concentrations of solid crustal particles, with relatively little associated H2SO4. Giant particles larger than 5 m were occasionally observed in this aerosol. The composition of this material closely matches that of bulk ash from the Mt. Augustine volcano, which erupted 9–13 days before collection of this sample. This brings forth the possibility that pockets of ash-rich aerosol existed over parts of south and central Alska during the AGASP-II field mission. There is no evidence that these volcanic aerosols were present in the AGASP study area north of the Brooks Range.  相似文献   

8.
A theory is offered for the drag and heat transfer relations in the statistically steady, horizontally homogeneous, diabatic, barotropic planetary boundary layer. The boundary layer is divided into three regionsR 1,R 2, andR 3, in which the heights are of the order of magnitude ofz 0,L, andh, respectively, wherez 0 is the roughness length for either momentum or temperature,L is the Obukhov length, andh is the height of the planetary boundary layer. A matching procedure is used in the overlap zones of regionsR 1 andR 2 and of regionsR 2 andR 3, assuming thatz 0 L h. The analysis yields the three similarity functionsA(),B(), andC() of the stability parameter, = u */fL, where is von Kármán's constant,u * is the friction velocity at the ground andf is the Coriolis parameter. The results are in agreement with those previously found by Zilitinkevich (1975) for the unstable case, and differ from his results only by the addition of a universal constant for the stable case. Some recent data from atmospheric measurements lend support to the theory and permit the approximate evaluation of universal constants.  相似文献   

9.
We present the first application of a multi-stage impactor to study volcanic particle emissions to the troposphere from Masaya volcano, Nicaragua. Concentrations of soluble SO4 2–,Cl–, F–, NO3 –, K+, Na+,NH4 +, Ca2+ and Mg2+ were determined in 11 size bins from 0.07 m to >25.5 m. The near-source size distributions showed major modes at 0.5m (SO4 2–, H+,NH4 +); 0.2 m and 5.0 m (Cl–) and 2.0–5.0 m(F–). K+ and Na+ mirrored the SO4 2– size-resolvedconcentrations closely, suggesting that these were transported primarily asK2SO4 and Na2SO4 in acidic solution, while Mg2+ andCa2+ presented modes in both <1 m and >1 m particles. Changes in relative humidity were studied by comparing daytime (transparent plume) and night-time (condensed plume) results. Enhanced particle growth rates were observed in the night-time plume as well as preferential scavenging of soluble gases, such as HCl, by condensed water. Neutralisation of the acidic aerosol by background ammonia was observed at the crater rim and to a greater extent approximately 15 km downwind of the active crater. We report measurements of re-suspended near-source volcanic dust, which may form a component of the plume downwind. Elevated levels ofSO4 2–, Cl–, F–,H+, Na+, K+ and Mg2+ were observed around the 10 m particle diameter in this dust. The volcanic SO4 2– flux leaving the craterwas 0.07 kg s–1.  相似文献   

10.
Ambient particulate sulfate measurements have been intermittently performed at a rural site in Israel over a period of more than two years. Concurrent measurements of ambient pollutants (SO2, NO–NOx, and O3), as well as meteorological data, were also carried out. The daily data included four particulate sulfate samples representing four successive 6 h accumulating periods. The measured concentrations of sulfate ions ranged from a low 2 g m-3 observed during the winter season to a high of >50 g m-3 obtained during the summer. Little correlation was obtained between the sulfate concentration and either O3 or SO2, although sulfate and O3 showed a similar diurnal and annual trend. Based on the data distribution and on a photochemical model, it was concluded that a large part of the particulate sulfate observed at the eastern coast of the Mediterranean Sea must be related to long-range transport from distant sources.  相似文献   

11.
The rainwater composition in the vicinity of Mainz, FRG, has been investigated with special emphasis on insoluble constituents. The number size distribution was determined in the range from 0.1 m up to 100 m radius. For particles with r>0.5 m radius the shape of the size distribution of insoluble particles in rain follows the shape of the average urban and rural aerosol. In this particular size range no major size selective removal processes could be seen. For r<0.5 m the number size distribution tends to flatten compared to the average aerosol. This might be the indication of a size selective removal process (Greenfield Gap).  相似文献   

12.
Separation of electrostatic charge during the transport of particles by wind adds a force to the gravitational and fluid forces that determine trajectories of particles moving by saltation. Evaluating this electrostatic force requires the electric field strength very near the saltation surface, and charge-to-mass ratios for the moving particles. Field mill readings 4 cm above the surface in a moderate blizzard showed electric field strength as high as +30 kV m-1. Another experiment gave charge-to-mass ratios of individual saltation particles in low-level drifting that ranged between +72 C kg-1 and -208 C kg-1. From these measurements, we estimated electrostatic forces as large as the gravitational force on some saltating particles. Including forces of this magnitude in the equations of motion significantly alters predicted saltation trajectories from those for uncharged particles. Predictions appear reasonable that for some saltating particles, the electrostatic force prevents new surface impacts. These results should help improve models of energy transfer in the planetary boundary layer during blizzards and sandstorms.  相似文献   

13.
Aerosol chemical composition and trace gas measurements were made at twolocations on the northeastern peninsula of Tenerife during the ACE-2HILLCLOUD experiment, between 28 June and 23 July 1997. Measurementswere made of coarse (#gt;2.5 m aerodynamic diameter) and fine (#lt; 2.5m) aerosol Cl–, NO3 –,SO4 2–, non-sea saltSO4 2– (NSSS),CH3SO3 – (MSA) andNH4 +, and gas phase dimethylsulphide (DMS), HCl,HNO3, SO2, CH3COOH, HCOOH andNH3. Size distributions were measured using a cascadeimpactor. Results show that in marine air masses NSSS and MSA wereformed via DMS oxidation, with additional NSSS present in air massescontaining a continental component. Using a Eulerian box model approachfor aerosols transported between upwind and downwind sites, a mean NSSSproduction rate of 4.36 × 10–4 gm–3 s–1 was calculated for daytimeclear sky periods (highest insolation), with values for cloudy periodsduring daytime and nighttime of 3.55 × 10–4 and2.40 × 10–4 g m–3s–1, respectively. The corresponding rates for MSA were6.23 × 10–6, 8.49 × 10–6and 6.95 × 10–6 g m–3s–1, respectively. Molar concentration ratios forMSA/NSSS were 8.7% (1.8–18.2%) and 1.9%(1.3–3.5%) in clean and polluted air masses, respectively.Reactions occurring within clouds appeared to have a greater influenceon rates of MSA production, than of NSSS, while conversely daytime gasphase reactions were more important for NSSS. For MSA, nighttimein-cloud oxidation rates exceeded rates of daytime gas phase productionvia OH oxidation of DMS. NSSS, MSA and ammonium had trimodal sizedistributions, with modes at 0.3, 4.0 and >10.0 m (NSSS andNH4 +), and 0.3, 1.5 and 4.0 m (MSA). Nosignificant production of other aerosol species was observed, with theexception of ammonium, which was formed at variable rates dependent onneutralisation of the aerosol with ammonia released from spatiallynon-uniform surface sources. Seasalt components were mainly present incoarse particles, although sub-micrometre chloride was also measured.Losses by deposition exceeded calculated expectations for all species,and were highest for the seasalt fraction and nitrate.  相似文献   

14.
Airborne measurements made during August 1985 over Greenland and its environs show that both accumulation-mode (0.1 m D2.0 m) and giant (D2 m) particles were present in relatively high concentrations in arctic haze layers and that the accumulation-mode particles dominated light scattering. Particles with diameters (D) between 1 and 4 m consisted predominately of mixed materials, small and dense inclusions, and probably organic compounds containing sulfur. Many of the particles from 0.1 to 1 m in diameter were also of mixed composition, with sulfuric acid, ammonium sulfate and organics probably the dominant constituents.  相似文献   

15.
Precipitation samples collected at Erdemli, Turkey, during February 1996–June 1997 were analysed to determine iron content and speciation. The purpose of the measurements was to examine the atmospheric abundance of iron and to quantify its solubility in the region. Spectrophotometric analyses of Fe(II) and reducible Fe(III) in precipitation samples, along with measurements of pH, conductivity, filterable iron (Fefilt), particulate aluminium (Alpar) and particulateiron (Fepar) were performed to determine iron solubility, which principally affects its bioavailability. Backward trajectories corresponding to the sampling dates were analysed to determine the sources of atmospheric constituents arriving at the site. Among these, the mineral dust transported from the Great Sahara to the region is considered to be a rich source of iron. The concentration of Fe(II) varied from below detection limit (0.02 M) up to 0.42 M,while the maximum concentration of total reactive Fe (referred as Fe(II) + reducible Fe(III) = Fereac) was found to be 1.0 M in precipitation. A strong correlation was found between particulate Fe and Al fractions, both of crustal origin. No correlation was observed between the soluble and insoluble fractions of iron. The soluble iron fraction, Fe(II) concentration varied independently from the concentrations of reducible Fe(III), Fefilt, Fepar, and from the pH of the precipitation. The Fefilt fraction (size < 0.45 m), measuredby Atomic Absorption Spectrophotometer, and frequently interpreted to be the soluble iron fraction in the literature, was found to be significantly higher than the corresponding Fereac fraction inprecipitation samples, most likely due to the colloidal iron content of the Fefilt fraction passing through the 0.45 m pore size filter. The volume weighted mean Fefilt concentration of the precipitation samples collected during the episodic `red rain' events was found to be relatively higher. The geometric mean ratios of soluble Fe(II) and of Fereac to Total Fe (Fefilt + Fepar), werefound to be 1.6% and 2.1%, respectively, while the mean ratioof Fefilt to Total Fe was 9.6%. The flux of bioavailable iron (Fereac)fraction in most atmospheric wet deposition events was found to be sufficient for supporting the maximum primary production rates that are typical for the Eastern Mediterranean Sea.  相似文献   

16.
Eighteen soil samples from central Sudan were fractionated by dry sieving ina size fraction from <45 m to >300 m while aerosols generatedfrom these soils were fractionated in the particle size range from 0.25 mto >16 m. The elemental concentrations of soil samples were determinedby energy-dispersive X-ray fluorescence, while the elemental concentrationsof generated aerosols were analysed by particle-induced X-ray emission. Theelements Al, K and Rb show a slight positive fractionation with decreasingparticle size throughout the particle size range studied. The concentrationsof Ca, Mn, Fe, Sr and Y are maximum in the small soil size fraction (<45m) and decrease for the coarse soil size fractions, while in the mineralaerosol particle sizes (0.25– > 16 m) the concentrations remainmore or less constant. The size distributions for Cr, Ti and Zr show a maximumin the particle size range 45–100 m and the concentrations of theseelements decrease sharply in the aerosol fraction down to 16 m to remainconstant in the smaller aerosol fractions.Enrichment factors for the elements were calculated relative to five referencematerials: average crustal rock, average soil, the investigated Sahara bulksoil, the finest fraction of this soil and the aerosol generated from thissoil, and using four reference elements: Al, Si, Ti and Fe. The enrichmentfactors were found to vary significantly depending on the choice of thereference material or the reference element. The enrichment factors for theSudan mineral aerosol were almost identical to those for Khartoum atmosphericaerosol but different from those for Namib mineral aerosol and Israelatmospheric aerosol following dust storms. Multivariate display methods(cluster analysis, principal component analysis and linear discriminantanalysis) were applied to the element ratios in the mineral aerosol from theSahara and Namib and this showed that these mineral aerosol can bedifferentiated into different groups. An attempt was also made to relate themineral aerosol to its parent soil through the use of these multivariatetechniques and the elemental ratios in both the mineral aerosols and the bulksoils (Namib and Sahara). It was also possible using the elemental ratios andthe multivariate display methods to associate the crustal component to themineral aerosol generated from the Sahara.  相似文献   

17.
Use of an airborne quartz crystal microbalance cascade impactor instrument together with a correlation spectrometer has allowed the flux of particles and their size distribution to be determined at Mount Erebus. The plume contributes 21±3 metric tomnes/day of aerosol particles to the Antarctic upper troposphere. The aerosol particles consist of larger (5–25 m) particles of elemental sulfur and silica, a middle sized group of iron oxides and smaller particles (less than 1 m) of complex liquids. Unlike many volcanic plumes, the Erebus plume has only a small amount of sulfate particles. The concentrations of particles in the Erebus plumes was 70–370 m/m3. Limited sampling of the Antarctic atmosphere at 8 km altitude but hundreds of km away from Erebus obtained a few large particles of sulfur and silicates, suggesting a similarity with the Erebus plume. The fallout of these particles occurs slowly over a broad area of the Antarctic continent.  相似文献   

18.
Rain and air of Florence have been collected in a continuous way andanalysed by flow analysis spectrofluorimetric methods for formaldehydeand hydrogen peroxide. Diurnal and seasonal variations were observed;the mean/maximum concentrations of all data (as gm–3) are 3.3/23.4 for HCHO and 0.4/4.93 forH2O2. The effect of external sources and ofphotochemical reactions produces periods of positive and negativecorrelations for these compounds. The mean/maximum rain concentration ofall data are 98/443 g l–1 for HCHO and 84/685 g l–1 for H2O2. Concentrationratios rain/air and discrepancies to Henry's Law equilibrium arediscussed.  相似文献   

19.
Two types of neutral planetary boundary layer (PBL) are distinguished:truly neutral – developed against a neutrally stratified free flow, and conventionally neutral – developed against a background stable stratification. Atmospheric PBLs treated asneutral are almost always conventionally neutral. Theoretical reasoning and results from large-eddy simulation (LES) show that A and B coefficients of the Rossby-number similarity theory are not constants. The same is true for thecoefficient Ch in the Rossby–Montgomery formula for the neutral boundary-layer depth h = Chu*/|f|, where u* is the friction velocity. Contrary to classical ideas, A, B and Ch depend on the ratio N N/|f| of the free-flow Brunt–V*auml;isäl ä frequency N to the absolute value of the Coriolis parameter |f|. This new development can explain why atmospheric and LES estimates of A, B and Ch appear inconsistent. It results from neglecting the fact that atmospheric data for N 102 were compared with LES data for N = 0, violating an obvious requirement of similarity with respect to N.  相似文献   

20.
On the determination of the height of the Ekman boundary layer   总被引：1，自引：1，他引：1  
The heighth of the Ekman turbulent boundary layer determined by the momentum flux profile is estimated with the aid of considerations of similarity and an analysis of the dynamic equations. Asymptotic formulae have been obtained showing that, with increasing instability,h increases as ¦¦1/2 (where is the non-dimensional stratification parameter); with increasing stability, on the other hand,h decreases as –1/2. For comparison, a simple estimate of the boundary-layer heighth u determined by the velocity profile is given. As is shown, in unstable stratification,h u behaves asymptotically as ¦¦–1, i.e., in a manner entirely different from that ofh .  相似文献   

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